Technical note: Absorption aerosol optical depth components from AERONET observations of mixed dust plumes

© Author(s) 2019.Absorption aerosol optical depth (AAOD) as obtained from sun–sky photometer measurements provides a measure of the light-absorbing properties of the columnar aerosol loading. However, it is not an unambiguous aerosol-type-specific parameter, particularly if several types of absorbing aerosols, for instance black carbon (BC) and mineral dust, are present in a mixed aerosol plume. The contribution of mineral dust to total aerosol light absorption is particularly important at UV wavelengths. In this study we refine a lidar-based technique applied to the separation of dust and non-dust aerosol types for the use with Aerosol Robotic Network (AERONET) direct sun and inversion products. We extend the methodology to retrieve AAOD related to non-dust aerosol (AAODnd) and BC (AAODBC). We test the method at selected AERONET sites that are frequently affected by aerosol plumes that contain a mixture of Saharan or Asian mineral dust and biomass-burning smoke or anthropogenic pollution, respectively. We find that aerosol optical depth (AOD) related to mineral dust as obtained with our methodology is frequently smaller than coarse-mode AOD. This suggests that the latter is not an ideal proxy for estimating the contribution of mineral dust to mixed dust plumes. We present the results of the AAODBC retrieval for the selected AERONET sites and compare them to coincident values provided in the Copernicus Atmosphere Monitoring System aerosol reanalysis.We find that modelled and AERONET AAODBC are most consistent for Asian sites or at Saharan sites with strong local anthropogenic sources.Peer reviewe

Constraining uncertainty in aerosol direct forcing

The uncertainty in present-day anthropogenic forcing is dominated by uncertainty in the strength of the contribution from aerosol. Much of the uncertainty in the direct aerosol forcing can be attributed to uncertainty in the anthropogenic fraction of aerosol in the present-day atmosphere, due to a lack of historical observations. Here we present a robust relationship between total present-day aerosol optical depth and the anthropogenic contribution across three multi-model ensembles and a large single-model perturbed parameter ensemble. Using observations of aerosol optical depth, we determine a reduced likely range of the anthropogenic component and hence a reduced uncertainty in the direct forcing of aerosol

Atmospheric aerosol attenuation effect on FD data analysis at the Pierre Auger Observatory

The atmospheric aerosol monitoring system of the Pierre Auger Observatory has been operating smoothly since 2004. Two laser facilities (Central Laser Facility, CLF and eXtreme Laser Facility, XLF) fire sets of 50 shots four times per hour during FD shifts to measure the highly variable hourly aerosol attenuation to correct the longitudinal UV light profiles of the Extensive Air Showers detected by the Fluorescence Detector. Hourly aerosol attenuation loads (Vertical Aerosol Optical Depth) are used to correct the measured profiles. Two techniques are used to determine the aerosol profiles, which have been proven to be fully compatible. The uncertainty in the VAOD profiles measured consequently leads to an uncertainty on the energy and on the estimation of the depth at the maximum development of a shower (X max ) of the event in analysis. To prove the validity of the aerosol attenuation measurements used in FD event analysis, the flatness of the ratio of reconstructed SD to FD energy as a function of the aerosol transmission to the depth of shower maximum has been verified.Comment: 6 pages, 10 figures, poster at UHECR 2018 (Paris, Oct 2018

Inverse Methods: a Powerful Tool for Evaluating Aerosol Data, Exemplified on Cases With Relevance for the Atmosphere and the Aerosol Climate Effect

For a complete description of a given aerosol, more than one parameter is necessary, e.g. parameters concerning size distribution, chemical composition, and particle morphology. On the other hand, most instruments measuring aerosol properties are sensitive mostly to one parameter, but cross-sensitive to others. These cross-sensitivities are often eliminated by assumptions during data evaluation, inducing systematic uncertainties in the results. The use of assumptions can be reduced by combining the information of several instruments on the same aerosol and using inverse methods for interpretation of the data. The presentation focuses on two application examples of these methods. The first example concerns a size distribution inversion algorithm that combines data from several instruments into one size distribution. The second example deals with an algorithm that retrieves the aerosol asymmetry parameter (with respect to particle scattering) from measurements of the aerosol absorption and spectral scattering and hemispheric backscattering coefficients, thereby providing a set of parameters that completely describes an aerosol with respect to its direct climate effect

Characterization and Quantification of Isoprene-Derived Epoxydiols in Ambient Aerosol in the Southeastern United States

Isoprene-derived epoxydiols (IEPOX) are identified in ambient aerosol samples for the first time, together with other previously identified isoprene tracers (i.e., 2-methyltetrols, 2-methylglyceric acid, C5-alkenetriols, and organosulfate derivatives of 2-methyltetrols). Fine ambient aerosol collected in downtown Atlanta, GA and rural Yorkville, GA during the 2008 August Mini-Intensive Gas and Aerosol Study (AMIGAS) was analyzed using both gas chromatography/quadrupole mass spectrometry (GC/MS) and gas chromatography/time-of-flight mass spectrometry (GC/TOFMS) with prior trimethylsilylation. Mass concentrations of IEPOX ranged from ~1 to 24 ng m^(−3) in the aerosol collected from the two sites. Detection of particle-phase IEPOX in the AMIGAS samples supports recent laboratory results that gas-phase IEPOX produced from the photooxidation of isoprene under low-NO_x conditions is a key precursor of ambient isoprene secondary organic aerosol (SOA) formation. On average, the sum of the mass concentrations of IEPOX and the measured isoprene SOA tracers accounted for about 3% of the organic carbon, demonstrating the significance of isoprene oxidation to the formation of ambient aerosol in this region

Aerosol meteorology of Maritime Continent for the 2012 7SEAS southwest monsoon intensive study - Part 2: Philippine receptor observations of fine-scale aerosol behavior

Abstract. The largest 7 Southeast Asian Studies (7SEAS) operations period within the Maritime Continent (MC) occurred in the August–September 2012 biomass burning season. Data included were observations aboard the M/Y Vasco, dispatched to the Palawan Archipelago and Sulu Sea of the Philippines for September 2012. At these locations, the Vasco observed MC smoke and pollution entering the southwest monsoon (SWM) monsoonal trough. Here we describe the research cruise findings and the finer-scale aerosol meteorology of this convectively active region. This 2012 cruise complemented a 2-week cruise in 2011 and was generally consistent with previous findings in terms of how smoke emission and transport related to monsoonal flows, tropical cyclones (TC), and the covariance between smoke transport events and the atmosphere's thermodynamic structure. Biomass burning plumes were usually mixed with significant amounts of anthropogenic pollution. Also key to aerosol behavior were squall lines and cold pools propagating across the South China Sea (SCS) and scavenging aerosol particles in their path. However, the 2012 cruise showed much higher modulation in aerosol frequency than its 2011 counterpart. Whereas in 2011 large synoptic-scale aerosol events transported high concentrations of smoke into the Philippines over days, in 2012 measured aerosol events exhibited a much shorter-term variation, sometimes only 3–12 h. Strong monsoonal flow reversals were also experienced in 2012. Nucleation events in cleaner and polluted conditions, as well as in urban plumes, were observed. Perhaps most interestingly, several cases of squall lines preceding major aerosol events were observed, as opposed to 2011 observations where these lines largely scavenged aerosol particles from the marine boundary layer. Combined, these observations indicate pockets of high and low particle counts that are not uncommon in the region. These perturbations are difficult to observe by satellite and very difficult to model. Indeed, the Navy Aerosol Analysis and Prediction System (NAAPS) simulations captured longer period aerosol events quite well but largely failed to capture the timing of high-frequency phenomena. Ultimately, the research findings of these cruises demonstrate the real world challenges of satellite-based missions, significant aerosol life cycle questions such as those the future Aerosol/Clouds/Ecosystems (ACE) will investigate, and the importance of small-scale phenomena such as sea breezes, squall lines, and nucleation events embedded within SWM patterns in dominating aerosol life cycle and potential relationships to clouds

Observations of heterogeneous reactions between Asian pollution and mineral dust over the Eastern North Pacific during INTEX-B

In-situ airborne measurements of trace gases, aerosol size distributions, chemistry and optical properties were conducted over Mexico and the Eastern North Pacific during MILAGRO and INTEX-B. Heterogeneous reactions between secondary aerosol precursor gases and mineral dust lead to sequestration of sulfur, nitrogen and chlorine in the supermicrometer particulate size range. Simultaneous measurements of aerosol size distributions and weak-acid soluble calcium result in an estimate of 11 wt% of CaCO_3 for Asian dust. During transport across the North Pacific, ~5–30% of the CaCO_3 is converted to CaSO_4 or Ca(NO_3)_2 with an additional ~4% consumed through reactions with HCl. The 1996 to 2008 record from the Mauna Loa Observatory confirm these findings, indicating that, on average, 19% of the CaCO_3 has reacted to form CaSO_4 and 7% has reacted to form Ca(NO_3)_2 and ~2% has reacted with HCl. In the nitrogen-oxide rich boundary layer near Mexico City up to 30% of the CaCO_3 has reacted to form Ca(NO_3)_2 while an additional 8% has reacted with HCl. These heterogeneous reactions can result in a ~3% increase in dust solubility which has an insignificant effect on their optical properties compared to their variability in-situ. However, competition between supermicrometer dust and submicrometer primary aerosol for condensing secondary aerosol species led to a 25% smaller number median diameter for the accumulation mode aerosol. A 10–25% reduction of accumulation mode number median diameter results in a 30–70% reduction in submicrometer light scattering at relative humidities in the 80–95% range. At 80% RH submicrometer light scattering is only reduced ~3% due to a higher mass fraction of hydrophobic refractory components in the dust-affected accumulation mode aerosol. Thus reducing the geometric mean diameter of the submicrometer aerosol has a much larger effect on aerosol optical properties than changes to the hygroscopic:hydrophobic mass fractions of the accumulation mode aerosol. In the presence of dust, nitric acid concentrations are reduced to 85% to 60–80% in the presence of dust. These observations support previous model studies which predict irreversible sequestration of reactive nitrogen species through heterogeneous reactions with mineral dust during long-range transport

The evolution of the global aerosol system in a transient climate simulation from 1860 to 2100

The evolution of the global aerosol system from 1860 to 2100 is investigated through a transient atmosphere-ocean General Circulation Model climate simulation with interactively coupled atmospheric aerosol and oceanic biogeochemistry modules. The microphysical aerosol module HAM incorporates the major global aerosol cycles with prognostic treatment of their composition, size distribution, and mixing state. Based on an SRES A1B emission scenario, the global mean sulfate burden is projected to peak in 2020 while black carbon and particulate organic matter show a lagged peak around 2070. From present day to future conditions the anthropogenic aerosol burden shifts generally from the northern high-latitudes to the developing low-latitude source regions with impacts on regional climate. Atmospheric residence- and aging-times show significant alterations under varying climatic and pollution conditions. Concurrently, the aerosol mixing state changes with an increasing aerosol mass fraction residing in the internally mixed accumulation mode. The associated increase in black carbon causes a more than threefold increase of its co-single scattering albedo from 1860 to 2100. Mid-visible aerosol optical depth increases from pre-industrial times, predominantly from the aerosol fine fraction, peaks at 0.26 around the sulfate peak in 2020 and maintains a high level thereafter, due to the continuing increase in carbonaceous aerosols. The global mean anthropogenic top of the atmosphere clear-sky short-wave direct aerosol radiative perturbation intensifies to −1.1 W m^−2 around 2020 and weakens after 2050 to −0.6 W m^−2, owing to an increase in atmospheric absorption. The demonstrated modifications in the aerosol residence- and aging-times, the microphysical state, and radiative properties challenge simplistic approaches to estimate the aerosol radiative effects from emission projections